Journal
SUSTAINABLE ENERGY & FUELS
Volume 5, Issue 1, Pages 117-126Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0se01314e
Keywords
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Funding
- German Federal Ministry of Education and Research (BMBF) within the Kopernikus Project P2X: Flexible use of renewable resources exploration, validation and implementation [FKZ 03SFK2A]
- German Federal Ministry of Education and Research (BMBF) within the project NaMoSyn (Nachhaltige Mobilitat durch synthetische Krafistoffe) [FKZ 03SF0566P0]
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The study presents an efficient non-oxidative synthesis of dimethoxymethane (DMM) using a bifunctional catalyst, highlighting the importance of catalyst selectivity under reaction conditions. The rapid evolution of DMM selectivity within the initial hours of operation demonstrates the potential cost and energy efficiency advantages of the method.
Dimethoxymethane (DMM), a promising synthetic fuel enabling clean combustion, is usually produced by condensation of methanol and formaldehyde, where the latter stems from methanol oxidation. Here, we report the hydrogen efficient non-oxidative DMM synthesis over a bifunctional Cu/zeolite catalyst in a continuous gas-phase fixed bed reactor. Methanol dehydrogenation to formaldehyde (FA) is coupled with FA condensation with methanol to yield DMM, hydrogen and water. Thermodynamic analysis confirms the general feasibility of this route and also manifests the vital importance of catalyst selectivity. Therein, close proximity of the catalyst's metallic Cu species and acidic sites is crucial. Noticeably, DMM selectivity of the catalyst only evolves within the first 13 hours of operation rising from 5.8 to 77.2%. A maximum DMM selectivity of 89.2 or 80.3% could be reached for 0.4 and 0.7 wt% Cu on Hb(836) zeolite with 1.9 or 3.6% methanol conversion, respectively. Comprehensive characterizations emphasize adaptation of Cu species and H beta zeolite under reaction conditions resulting in the decisive weakened dehydrogenation and condensation ability for high DMM selectivity. Process simulations confirm superior exergy efficiency compared to state-of-the-art technologies for DMM production already with the herein developed catalyst and highlights the high potential of further innovations for technical implementation.
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